改性赤泥吸附剂吸附低浓度CO2研究

以赤泥(RM)为原料,采用酸碱预处理方法制备了介孔赤泥材料(MRM),并以其为载体,利用浸渍法负载MgO以期增加碱性活性位点,通过BET,XRF,XRD,CO₂-TPD等手段对其结构和组成成分进行表征分析.研究表明,MRM的比表面积较RM提高了约28倍,孔结构丰富,物相组成分析表明以赤铁矿为主.负载MgO后,孔结构被堵塞,其比表面积和孔容随着Mg负载量的增加而减小,对5%MgO/MRM吸附剂通过XRD检测结果未发现MgO,表明Mg在吸附剂中分散性较好.当吸附温度为30℃,酸碱预处理赤泥的CO₂吸附容量为1.54mg/g,而5%MgO/MRM的吸附容量为2.26mg/g,说明负载MgO后,碱性活性位点数量明显增加,化学吸附作用增强,随着温度的升高,吸附容量逐渐降低.CO₂-TPD测试结果表明,MRM和5%MgO/MRM均以化学吸附为主,主要形成碳酸盐和碳酸氢盐结构.     

树脂基固态胺吸附材料的选择性CO2吸附性能

基于简单的湿浸渍法将聚乙烯亚胺(PEI)有效负载到多孔树脂(HP20)中,制备获得树脂基固态胺吸附材料,并探究了PEI负载量(30%~60%)、吸附温度(30~90℃)和压力(2~100kPa)对材料CO₂吸附性能的影响.研究表明树脂基固态胺吸附材料的最佳PEI负载量为50%,过量的PEI会致使材料CO₂吸附容量和胺基利用效率的显著降低.所筛选的材料在较低或较高的CO₂分压范围内均能展现出优异的CO₂吸附性能,在30℃下的CO₂吸附容量达到3.06~3.78mmol/g,表明该材料在不同CO₂分压的多种碳捕集应用中均有着较好的适用性.此外,树脂基固态胺吸附材料的CO₂/CH₄和CO₂/N₂选择性在2~100kPa的压力范围内分别有262~5858和708~11551,在各类传统或新兴的固体吸附材料中处于较高水平.     

树脂基固态胺吸附剂室温下对低浓度CO2的吸附性能研究

以大孔甲基丙烯酸酯吸附树脂为载体,聚乙烯亚胺(PEI)为有机胺,采用液相浸渍法制备出固态胺吸附剂,并研究了其在室温下对低浓度CO2的吸附行为.同时,利用氮气吸附、热重分析和扫描电镜表征了材料的物理化学性质,并采用热重法和固定床吸附法考察了材料的CO2吸附性能.结果表明,大孔树脂担载50%PEI(质量分数)时吸附性能最佳,对纯CO2的最大吸附量为175 mg·g-1;CO2的吸附行为由扩散动力学与吸附热力学共同决定,低温有利于提高吸附容量;吸附剂对400 ppm~15%浓度的CO2都具有优异的动态吸附性能,其中对400 ppm CO2的吸附量达到86 mg·g-1,对15%CO2的吸附量达到150 mg·g-1;湿度对吸附起促进作用,相对湿度为10%时,对400 ppm CO2的吸附量提高至139mg·g-1;吸附剂具有优异的循环性能,具有直接空气捕集CO2的潜力.     

CO2气氛热解与硝酸改性的生物炭Pb2+吸附性能对比

酸改性处理常被用于生物炭的改性过程,但也存在酸消耗量大、废液处理难和成本高等问题.利用热解过程直接改性提高生物炭重金属的去除效果、降低改性成本,是未来实现改性生物炭广泛使用的重要前提.为评估CO₂气氛热解法在生物炭制备和应用方面的优势和潜力,对CO₂气氛热解与HNO₃改性生物炭对Pb²⁺的去除性能进行对比分析.采用元素分析、傅里叶红外光谱(FTIR)和X射线光电子能谱(XPS)对生物炭的元素组成和结构特性进行表征.结果表明,500℃热解条件下,HNO₃改性的生物炭产生了较多的C=O和O=C—O—等羧基类官能团,并引入了—NO₍2(asy))和—NO₍2(sym))基团,提高了生物炭的表面活性和络合能力.CO₂气氛制备生物炭中含有较多的金属碳酸盐,可通过离子交换和共沉淀作用吸附去除Pb²⁺.此外,CO₂改性生物炭具有较大的比表面积和更优的微孔结构,有利于Pb^2+...     

葡萄树基活性炭的制备及其CO2吸附特性

为探讨葡萄树基活性炭在碳捕集与封存领域中的潜力,分别以葡萄树枝和树皮为原料采用CO₂活化法在800℃下制备了葡萄树枝基活性炭和葡萄树皮基活性炭,根据N₂物理吸附法计算了比表面积,用二维非定域密度函数理论（2D-NLDFT）分析了孔径分布特性,并使用热重分析法表征了两种活性炭的热解特性以及30℃的CO₂吸附特性.结果表明:①葡萄树枝基活性炭具有微孔结构,微孔孔径在0.36~1.6 nm之间,孔径为0.66 nm的微孔最多;葡萄树皮基活性炭具有大量微孔和少量中孔,孔径主要集中在0.36~1.9 nm之间.②葡萄树枝基和葡萄树皮基活性炭的CO₂吸附容量分别为1.096和0.247 mmol/g.③两种活性炭的CO₂吸附以物理吸附为主,其CO₂饱和产物在45℃前释放全部CO₂,葡萄树枝基活性炭的CO₂饱和产物较葡萄树皮基活性炭的CO₂饱和产物难于释放CO₂.④两种活性炭吸附CO₂后,在热重特性上出现的微量变化表明活性炭物质结构上的变化.研究显示,葡萄树枝基活性炭是一种良好的CO₂捕集材料,但其CO₂吸附容量比其他同类活性炭低,CO₂吸附量较高的葡萄树基活性炭的制备条件和改性方法需要进一步研究.      

氨基离子液体负载活性炭CO2吸附性能的负协同效应

通过三亚乙基四胺与L-乳酸的酸碱中和反应合成[TETA][L]离子液体,并将不同质量分数的离子液体负载到椰壳活性炭中,利用傅里叶红外光谱仪、X射线衍射仪、全自动比表面和孔径分布分析仪研究[TETA][L]离子液体浸渍对椰壳活性炭微观结构以及CO₂吸附性能的影响。结果表明:离子液体与活性炭之间的相互作用会导致石墨微晶细晶化,对活性炭的结构稳定性有不利影响,而离子液体对椰壳活性炭孔隙结构的"堵塞式"填充,导致复合材料CO₂物理吸附性能显著下降和CO₂化学吸附性能有限增加,这是造成复合材料CO₂总吸收性能显著降低的根本原因,且离子液体在活性炭中呈现了一种由小孔径到大孔径的"阶梯式"填充行为。     

SO2对掺杂KMnO4的K2CO3/Al2O3吸附剂脱碳性能影响

针对SO₂对吸附剂CO₂吸附性能的影响,该文采用溶胶-凝胶法制备氧化铝气凝胶载体,浸渍法制备吸附剂,通过固定床实验系统进行N₂低温吸附-脱附实验,研究了掺杂KMnO₄的K₂CO₃/Al₂O₃吸附剂CO₂吸附性能以及SO₂对吸附剂吸附性能的影响。利用Avrami模型计算吸附动力学,并结合吸附剂的孔隙和晶相结构变化分析吸附机理。结果表明：吸附实验最佳反应温度60℃,掺杂KMnO₄提高了K₂CO₃/Al₂O₃的CO₂吸附性能,吸附量提高0.13 mmol/g。在CO₂吸附实验中加入微量SO₂,掺杂KMnO₄后会减小烟气中SO₂对CO₂吸附...     

PEI改性生物炭的制备及对CO2吸附性能的评价

采用超声辅助-水热法将聚乙烯亚胺（PEI）成功接枝到玉米芯生物炭表面,制备了PEI改性生物炭材料（PBC）,并通过X射线衍射（XRD）、扫描电子显微镜（SEM）、比表面积分析仪和傅里叶红外光谱仪（FTIR）等方法对其表征.结果表明,虽然PEI通过CN、C-N和离子键与生物炭表面的活性基团链接,但制备的PBC材料仍保持原生炭的无定型结构和形貌,且比表面积高达928.1 m²·g^-1.同时,还研究了PBC的吸附性能和热力学行为,结果表明,吸附过程符合Langmuir等温吸附机制,属于微孔单层吸附过程,而且随温度的降低,吸附量增大,在10、20和30℃时,饱和吸附量（Q_m）分别为6.47、4.75和2.64 mmol·g^-1.此外,PBC重复利用性能良好,容易实现热再生,即使循环利用10次,吸附性能也无显著变化（p>0.05）,且穿透吸附量（Q_B）保持在2.6~2.7 mmol·g^-1.     

石墨烯量子点辅助合成Cu-MOFs及CO2吸附行为

选用一种成本低、可大规模合成的Cu基MOFs（Cu-MOFs）材料作为CO₂吸附剂,在原位合成过程中添加石墨烯量子点以调控其晶体结构.结果表明：适量石墨烯量子点的添加有利于提高Cu-MOFs的比表面积和孔体积,相比未改性MOFs材料,改性后的CO₂吸附性能有所提高,25℃,100kPa时提高了4.5%.随着温度升高,吸附容量提升越明显.改性后的MOFs对于N₂的吸附量则比未改性时更低,因此计算得到的CO₂/N₂吸附选择性也更高,增加了近一倍.综合等量吸附热的考察结果发现,尤其添加适量含N石墨烯量子点的Cu-MOFs吸附剂不仅具备了较高的吸附容量、吸附选择性,还展现了较理想的吸附热,因此兼具了较优CO₂吸附性能和较低脱附能耗的特点,为MOFs吸附剂的改性提供了一点参考价值.     

O2/CO2气氛下氮反应机理的研究

选取CH4、O2、CO2、Ar、NO、NH3，等气体，作为混合气和煤粉一起送入一维沉降炉内，以模拟O2／CO2气氛下煤中燃料氮、循环NO以及二者的相互作用对NO排放的影响，结果显示，在还原性气氛下NH3、HCN、CH4、CO与循环NO间的反应是NO排放下降的主要因素，且煤焦与NO的异相反应、吸附反应对NO的降解效果要明显高于氧化性气氛，同时，CO2体积分数的增加使得燃料中氮的氧化率升高，循环NO的降解率下降；氧化性气氛下随CO2体积分数的增加，燃料中氮的氧化率也增加，但循环NO的降解率升高．当CO2体积分数不变时，其对NO降解的作用随循环NO体积分数的增加愈加明显，在循环NO也不变且CO2体积分数较低时，随过量空气系数的增加，循环NO的降解率下降，而CO2体积分数较高时则出现相反情况。     

负载量对氨水吸收CO2的影响规律及添加剂的作用研究

进行了氨法脱碳过程中吸收剂中CO2负载量对CO2脱除率影响的实验研究.结果发现,CO2脱除率随着负载量的增大而显著减小,高负载量(≥0.4)时,增加吸收液中总氨质量分数(吸收液中所有包含氨分子和铵离子的物质,并统一换算成NH3的质量分数)并不能有效地提高CO2的脱除率.同时,分别对有机和无机添加剂进行筛选,选取哌嗪(P...     

MgO-based adsorbents for CO2 adsorption: Influence of structural and textural properties on the CO2 adsorption performance

A series of MgO-based adsorbents were prepared through solution–combustion synthesis and ball-milling process.The prepared MgO-based powders were characterized using X-ray diffraction,scanning electron microscopy,N_2 physisorption measurements,and employed as potential adsorbents for CO_2 adsorption.The influence of structural and textural properties of these adsorbents over the CO_2 adsorption behaviour was also investigated.The results showed that MgO-based products prepared by solution–combustion and ball-milling processes,were highly porous,fluffy,nanocrystalline structures in nature,which are unique physico-chemical properties that significantly contribute to enhance their CO_2 adsorption.It was found that the MgO synthesized by solution combustion process,using a molar ratio of urea to magnesium nitrate(2:1),and treated by ball-milling during 2.5 hr(MgO-BM2.5h),exhibited the maximum CO_2 adsorption capacity of 1.611 mmol/g at 25℃ and 1 atm,mainly via chemisorption.The CO_2 adsorption behaviour on the MgO-based adsorbents was correlated to their improved specific surface area,total pore volume,pore size distribution and crystallinity.The reusability of synthesized MgO-BM2.5h was confirmed by five consecutive CO_2adsorption–desorption times,without any significant loss of performance,that supports the potential of MgO-based adsorbent.The results confirmed that the special features of MgO prepared by solution–combustion and treated by ball-milling during 2.5 hr are favorable to be used as effective MgO-based adsorbent in post-combustion CO_2 capture technologies.     

胺基官能基化的HMS吸附水体中的腐殖酸

研究了胺基表面官能化前后的HMS(hexagonal mesoporous silica)对腐殖酸的吸附, Freundlich方程拟合结果表明,表面官能化后吸附常数K值由0.56提高至105,反映出表面官能化能显著改善HMS对腐殖酸的吸附,且低pH值条件下吸附效果更佳.表征结果显示,腐殖酸分子主要吸附在表面胺化HMS的中孔孔道内,并首先占据吸附剂中较大的中孔孔道.吸附动力学结果显示腐殖酸在表面胺化的HMS上吸附符合二级动力学,吸附速率主要受孔道内扩散控制.     

Breakthrough CO2 adsorption in bio-based activated carbons

In this work, the effects of different methods of activation on CO₂ adsorption performance of activated carbon were studied. Activated carbons were prepared from biochar, obtained from fast pyrolysis of white wood, using three different activation methods of steam activation, CO₂ activation and Potassium hydroxide (KOH) activation. CO₂ adsorption behavior of the produced activated carbons was studied in a fixed-bed reactor set-up at atmospheric pressure, temperature range of 25–65°C and inlet CO₂ concentration range of 10–30 mol% in He to determine the effects of the surface area, porosity and surface chemistry on adsorption capacity of the samples. Characterization of the micropore and mesopore texture was carried out using N₂ and CO₂ adsorption at 77 and 273 K, respectively. Central composite design was used to evaluate the combined effects of temperature and concentration of CO₂ on the adsorption behavior of the adsorbents. The KOH activated carbon with a total micropore volume of 0.62 cm³/g and surface area of 1400 m²/g had the highest CO₂ adsorption capacity of 1.8 mol/kg due to its microporous structure and high surface area under the optimized experimental conditions of 30 mol% CO₂ and 25°C. The performance of the adsorbents in multi-cyclic adsorption process was also assessed and the adsorption capacity of KOH and CO₂ activated carbons remained remarkably stable after 50 cycles with low temperature (160°C) regeneration.     

CO2 adsorption using TiO2 composite polymeric membranes: A kinetic study

CO₂ is the main greenhouse gas which causes global climatic changes on larger scale. Many techniques have been utilised to capture CO₂. Membrane gas separation is a fast growing CO₂ capture technique, particularly gas separation by composite membranes. The separation of CO₂ by a membrane is not just a process to physically sieve out of CO₂ through the controlled membrane pore size. It mainly depends upon diffusion and solubility of gases, particularly for composite dense membranes. The blended components in composite membranes have a high capability to adsorb CO₂. The adsorption kinetics of the gases may directly affect diffusion and solubility. In this study, we have investigated the adsorption behaviour of CO₂ in pure and composite membranes to explore the complete understanding of diffusion and solubility of CO₂ through membranes. Pure cellulose acetate (CA) and cellulose acetate-titania nanoparticle (CA-TiO₂) composite membranes were fabricated and characterised using SEM and FTIR analysis. The results indicated that the blended CA-TiO₂ membrane adsorbed more quantity of CO₂ gas as compared to pure CA membrane. The high CO₂ adsorption capacity may enhance the diffusion and solubility of CO₂ in the CA-TiO₂ composite membrane, which results in a better CO₂ separation. The experimental data was modelled by Pseudo first-order, pseudo second order and intra particle diffusion models. According to correlation factor R², the Pseudo second order model was fitted well with experimental data. The intra particle diffusion model revealed that adsorption in dense membranes was not solely consisting of intra particle diffusion.     

不同特性的多孔炭对CO2的吸附研究

分别用苯胺和糠醇为碳源、NaY分子筛为硬模板在碳化温度为700与900℃下合成了多孔炭(MC-AN-700、MC-AN-900、MC-FA-700和MC-FA-900),并对材料进行了结构表征,研究了低浓度CO2在这些材料和商业活性炭(AC)上的动态吸附.结果显示,MC-AN-700的氮和氧的含量均最高,分别为6.59%和8.71%;MC-FA-900的总孔容居于首位,为0.73cm3/g,但微孔体积中,AC的最大,为0.35cm3/g.在常温常压下,初始浓度为10%的 CO2在5种材料上的饱和吸附量的顺序为:MC-AN-700(2.20mmol/g)>MC-AN- 900(1.72mmol/g)>AC(1.59mmol/g)>MC-FA-900(1.45mmol/g)>MC-FA-700(1.09mmol/g),吸附差异受吸附剂的微孔孔容和氮含量共同影响.在2%~10%的范围内,CO2吸附量随初始浓度增加而增加;在20、45和65℃3个温度下,CO2吸附量随温度升高而降低.经4次脱附再生后,MC-AN-700的吸附量仍保持了原有吸附量的91%,高于MC-FA-900(86%)与AC(85%).